Chemically coupling SnO 2 quantum dots and MXene for efficient CO 2 electroreduction to formate and Zn–CO 2 battery

Author:

Han Lili12ORCID,Peng Xianyun3,Wang Hsiao-Tsu45ORCID,Ou Pengfei6,Mi Yuying7,Pao Chih-Wen8,Zhou Jigang9ORCID,Wang Jian9ORCID,Liu Xijun7,Pong Way-Faung5,Song Jun6,Lin Zhang10ORCID,Luo Jun7ORCID,Xin Huolin L.1ORCID

Affiliation:

1. Department of Physics and Astronomy, University of California, Irvine, CA 92697

2. State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China

3. Institute of Zhejiang University-Quzhou, Quzhou 324000, China

4. Bachelor's Program in Advanced Materials Science, Tamkang University, New Taipei City 25137, Taiwan

5. Department of Physics, Tamkang University, New Taipei City 25137, Taiwan

6. Department of Mining and Materials Engineering, McGill University, Montreal, QC H3A 0C5, Canada

7. Institute for New Energy Materials & Low-Carbon Technologies and Tianjin Key Lab of Photoelectric Materials & Devices, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China

8. National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan

9. Canadian Light Source Inc., University of Saskatchewan, Saskatoon, SK S7N 2V3, Canada

10. School of Metallurgy and Environment, Central South University, Changsha 410083, China

Abstract

Electrochemical conversion of CO 2 into formate is a promising strategy for mitigating the energy and environmental crisis, but simultaneously achieving high selectivity and activity of electrocatalysts remains challenging. Here, we report low-dimensional SnO 2 quantum dots chemically coupled with ultrathin Ti 3 C 2 T x MXene nanosheets (SnO 2 /MXene) that boost the CO 2 conversion. The coupling structure is well visualized and verified by high-resolution electron tomography together with nanoscale scanning transmission X-ray microscopy and ptychography imaging. The catalyst achieves a large partial current density of −57.8 mA cm −2 and high Faradaic efficiency of 94% for formate formation. Additionally, the SnO 2 /MXene cathode shows excellent Zn–CO 2 battery performance, with a maximum power density of 4.28 mW cm −2 , an open-circuit voltage of 0.83 V, and superior rechargeability of 60 h. In situ X-ray absorption spectroscopy analysis and first-principles calculations reveal that this remarkable performance is attributed to the unique and stable structure of the SnO 2 /MXene, which can significantly reduce the reaction energy of CO 2 hydrogenation to formate by increasing the surface coverage of adsorbed hydrogen.

Funder

National Science Foundation

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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